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Temperature-Dependent Nitrous Oxide/Carbon Dioxide Preferential Adsorption in a Thiazolium-Functionalized NU-1000 Metal–Organic Framework
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-12-02 , DOI: 10.1021/acsami.1c21437 Giorgio Mercuri 1 , Marco Moroni 2 , Simona Galli 2 , Giulia Tuci 1 , Giuliano Giambastiani 1, 3 , Tongan Yan 4 , Dahuan Liu 4 , Andrea Rossin 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-12-02 , DOI: 10.1021/acsami.1c21437 Giorgio Mercuri 1 , Marco Moroni 2 , Simona Galli 2 , Giulia Tuci 1 , Giuliano Giambastiani 1, 3 , Tongan Yan 4 , Dahuan Liu 4 , Andrea Rossin 1
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Solvent-assisted ligand incorporation (SALI) of the ditopic linker 5-carboxy-3-(4-carboxybenzyl)thiazolium bromide [(H2PhTz)Br] into the zirconium metal–organic framework NU-1000 [Zr6O4(OH)8(H2O)4(TBAPy)2, where NU = Northwestern University and H4TBAPy = 1,3,6,8-tetrakis(p-benzoic-acid)pyrene], led to the SALIed NU-1000-PhTz material of minimal formula [Zr6O4(OH)6(H2O)2(TBAPy)2(PhTz)]Br. NU-1000-PhTz has been thoroughly characterized in the solid state. As confirmed by powder X-ray diffraction, this material keeps the same three-dimensional architecture of NU-1000 and the dicarboxylic extra linker bridges adjacent [Zr6] nodes ca. 8 Å far apart along the crystallographic c-axis. The functionalized MOF has a BET specific surface area of 1560 m2/g, and it is featured by a slightly higher thermal stability than its parent material (Tdec = 820 vs. 800 K, respectively). NU-1000-PhTz has been exploited for the capture and separation of two pollutant gases: carbon dioxide (CO2) and nitrous oxide (N2O). The high thermodynamic affinity for both gases [isosteric heat of adsorption (Qst) = 25 and 27 kJ mol–1 for CO2 and N2O, respectively] reasonably stems from the strong interactions between these (polar) “stick-like” molecules and the ionic framework. Intriguingly, NU-1000-PhTz shows an unprecedented temperature-dependent adsorption capacity, loading more N2O in the 298 K ≤ T ≤ 313 K range but more CO2 at temperatures falling out of this range. Grand canonical Monte Carlo simulations of the adsorption isotherms confirmed that the preferential adsorption sites of both gases are the triangular channels (micropores) in close proximity to the polar pillar. While CO2 interacts with the thiazolium ring in an “end-on” fashion through its O atoms, N2O adopts a “side-on” configuration through its three atoms simultaneously. These findings open new horizons in the discovery of functional materials that may discriminate between polluting gases through selective adsorption at different temperatures.
中文翻译：
噻唑鎓官能化 NU-1000 金属-有机骨架中的温度依赖性一氧化二氮/二氧化碳优先吸附
溶剂辅助配体掺入 (SALI) 双位连接体 5-羧基-3-(4-羧基苄基) 噻唑溴化物 [( H 2 PhTz )Br] 进入锆金属-有机框架NU-1000 [Zr 6 O 4 (OH ) 8 (H 2 O) 4 (TBAPy) 2，其中 NU = 西北大学和 H 4 TBAPy = 1,3,6,8-四（对苯甲酸）芘]，导致 SALIed NU-1000- PhTz材料最小分子式[Zr 6 O 4 (OH) 6 (H 2 O) 2 (TBAPy) 2( PhTz )]Br。NU-1000-PhTz已在固态进行了彻底的表征。正如粉末 X 射线衍射所证实的那样，这种材料保持了与NU-1000相同的三维结构，并且二羧酸额外接头桥接了相邻的 [Zr 6 ] 节点。沿晶体学c轴相距 8 Å 。功能化 MOF 的 BET 比表面积为 1560 m 2 /g，其热稳定性略高于其母材（T dec = 820 vs. 800 K）。NU-1000-PhTz已被用于捕获和分离两种污染气体：二氧化碳 (CO 2 ) 和一氧化二氮 (N 2 O)。两种气体的高热力学亲和力 [ CO 2和 N 2 O 的等量吸附热 ( Q st ) = 25 和 27 kJ mol –1 ] 合理地源于这些（极性）“棒状”之间的强相互作用分子和离子框架。有趣的是，NU-1000-PhTz显示出前所未有的温度依赖性吸附能力，在 298 K ≤ T ≤ 313 K 范围内负载更多的 N 2 O，但更多的 CO 2在超出此范围的温度下。吸附等温线的大规范蒙特卡罗模拟证实，两种气体的优先吸附位点都是靠近极柱的三角形通道（微孔）。CO 2通过其 O 原子以“端接”方式与噻唑环相互作用，而 N 2 O 通过其三个原子同时采用“侧接”配置。这些发现为发现功能材料开辟了新的视野，这些材料可以通过在不同温度下的选择性吸附来区分污染气体。
更新日期：2021-12-15
中文翻译：
噻唑鎓官能化 NU-1000 金属-有机骨架中的温度依赖性一氧化二氮/二氧化碳优先吸附
溶剂辅助配体掺入 (SALI) 双位连接体 5-羧基-3-(4-羧基苄基) 噻唑溴化物 [( H 2 PhTz )Br] 进入锆金属-有机框架NU-1000 [Zr 6 O 4 (OH ) 8 (H 2 O) 4 (TBAPy) 2，其中 NU = 西北大学和 H 4 TBAPy = 1,3,6,8-四（对苯甲酸）芘]，导致 SALIed NU-1000- PhTz材料最小分子式[Zr 6 O 4 (OH) 6 (H 2 O) 2 (TBAPy) 2( PhTz )]Br。NU-1000-PhTz已在固态进行了彻底的表征。正如粉末 X 射线衍射所证实的那样，这种材料保持了与NU-1000相同的三维结构，并且二羧酸额外接头桥接了相邻的 [Zr 6 ] 节点。沿晶体学c轴相距 8 Å 。功能化 MOF 的 BET 比表面积为 1560 m 2 /g，其热稳定性略高于其母材（T dec = 820 vs. 800 K）。NU-1000-PhTz已被用于捕获和分离两种污染气体：二氧化碳 (CO 2 ) 和一氧化二氮 (N 2 O)。两种气体的高热力学亲和力 [ CO 2和 N 2 O 的等量吸附热 ( Q st ) = 25 和 27 kJ mol –1 ] 合理地源于这些（极性）“棒状”之间的强相互作用分子和离子框架。有趣的是，NU-1000-PhTz显示出前所未有的温度依赖性吸附能力，在 298 K ≤ T ≤ 313 K 范围内负载更多的 N 2 O，但更多的 CO 2在超出此范围的温度下。吸附等温线的大规范蒙特卡罗模拟证实，两种气体的优先吸附位点都是靠近极柱的三角形通道（微孔）。CO 2通过其 O 原子以“端接”方式与噻唑环相互作用，而 N 2 O 通过其三个原子同时采用“侧接”配置。这些发现为发现功能材料开辟了新的视野，这些材料可以通过在不同温度下的选择性吸附来区分污染气体。
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